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Title: Enhancing catalytic performance of dilute metal alloy nanomaterials

Abstract

Dilute alloys are promising materials for sustainable chemical production; however, their composition and structure affect their performance. Herein, a comprehensive study of the effects of pretreatment conditions on the materials properties of Pd0.04Au0.96 nanoparticles partially embedded in porous silica is related to the activity for catalytic hydrogenation of 1-hexyne to 1-hexene. A combination of in situ characterization and theoretical calculations provide evidence that changes in palladium surface content are induced by treatment in oxygen, hydrogen and carbon monoxide at various temperatures. In turn, there are changes in hydrogenation activity because surface palladium is necessary for H2 dissociation. These Pd0.04Au0.96 nanoparticles in the porous silica remain structurally intact under many cycles of activation and deactivation and are remarkably resistant to sintering, demonstrating that dilute alloy catalysts are highly dynamic systems that can be tuned and maintained in a active state.

Authors:
 [1];  [2];  [1]; ORCiD logo [3]; ORCiD logo [2];  [1];  [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [3];  [1]; ORCiD logo [4]; ORCiD logo [1]
  1. Harvard Univ., Cambridge, MA (United States)
  2. Stony Brook Univ., NY (United States)
  3. Univ. of Pennsylvania, Philadelphia, PA (United States)
  4. Stony Brook Univ., NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Integrated Mesoscale Architectures for Sustainable Catalysis (IMASC); Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
OSTI Identifier:
1616944
Report Number(s):
BNL-215897-2020-JAAM
Journal ID: ISSN 2399-3669
Grant/Contract Number:  
SC0012704; SC0012573; NNCI-1542153; DMR-1720530
Resource Type:
Accepted Manuscript
Journal Name:
Communications Chemistry
Additional Journal Information:
Journal Volume: 3; Journal Issue: 1; Journal ID: ISSN 2399-3669
Publisher:
Springer Nature
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE

Citation Formats

Luneau, Mathilde, Guan, Erjia, Chen, Wei, Foucher, Alexandre C., Marcella, Nicholas, Shirman, Tanya, Verbart, David M. A., Aizenberg, Joanna, Aizenberg, Michael, Stach, Eric A., Madix, Robert J., Frenkel, Anatoly I., and Friend, Cynthia M. Enhancing catalytic performance of dilute metal alloy nanomaterials. United States: N. p., 2020. Web. doi:10.1038/s42004-020-0293-2.
Luneau, Mathilde, Guan, Erjia, Chen, Wei, Foucher, Alexandre C., Marcella, Nicholas, Shirman, Tanya, Verbart, David M. A., Aizenberg, Joanna, Aizenberg, Michael, Stach, Eric A., Madix, Robert J., Frenkel, Anatoly I., & Friend, Cynthia M. Enhancing catalytic performance of dilute metal alloy nanomaterials. United States. doi:https://doi.org/10.1038/s42004-020-0293-2
Luneau, Mathilde, Guan, Erjia, Chen, Wei, Foucher, Alexandre C., Marcella, Nicholas, Shirman, Tanya, Verbart, David M. A., Aizenberg, Joanna, Aizenberg, Michael, Stach, Eric A., Madix, Robert J., Frenkel, Anatoly I., and Friend, Cynthia M. Thu . "Enhancing catalytic performance of dilute metal alloy nanomaterials". United States. doi:https://doi.org/10.1038/s42004-020-0293-2. https://www.osti.gov/servlets/purl/1616944.
@article{osti_1616944,
title = {Enhancing catalytic performance of dilute metal alloy nanomaterials},
author = {Luneau, Mathilde and Guan, Erjia and Chen, Wei and Foucher, Alexandre C. and Marcella, Nicholas and Shirman, Tanya and Verbart, David M. A. and Aizenberg, Joanna and Aizenberg, Michael and Stach, Eric A. and Madix, Robert J. and Frenkel, Anatoly I. and Friend, Cynthia M.},
abstractNote = {Dilute alloys are promising materials for sustainable chemical production; however, their composition and structure affect their performance. Herein, a comprehensive study of the effects of pretreatment conditions on the materials properties of Pd0.04Au0.96 nanoparticles partially embedded in porous silica is related to the activity for catalytic hydrogenation of 1-hexyne to 1-hexene. A combination of in situ characterization and theoretical calculations provide evidence that changes in palladium surface content are induced by treatment in oxygen, hydrogen and carbon monoxide at various temperatures. In turn, there are changes in hydrogenation activity because surface palladium is necessary for H2 dissociation. These Pd0.04Au0.96 nanoparticles in the porous silica remain structurally intact under many cycles of activation and deactivation and are remarkably resistant to sintering, demonstrating that dilute alloy catalysts are highly dynamic systems that can be tuned and maintained in a active state.},
doi = {10.1038/s42004-020-0293-2},
journal = {Communications Chemistry},
number = 1,
volume = 3,
place = {United States},
year = {2020},
month = {4}
}

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